Exact Simulation of Pigment-Protein Complexes Unveils Vibronic
Renormalization of Electronic Parameters in Ultrafast Spectroscopy
- URL: http://arxiv.org/abs/2106.14286v2
- Date: Sun, 5 Jun 2022 17:29:41 GMT
- Title: Exact Simulation of Pigment-Protein Complexes Unveils Vibronic
Renormalization of Electronic Parameters in Ultrafast Spectroscopy
- Authors: F. Caycedo-Soler, A. Mattioni, J. Lim, T. Renger, S. F. Huelga, M. B.
Plenio
- Abstract summary: Primary steps of photosynthesis rely on the generation, transport, and trapping of excitons in pigment-protein complexes (PPCs)
PPCs possess highly structured vibrational spectra, combining many discrete intra-pigment modes and a quasi-continuous of protein modes, with vibrational and electronic couplings of comparable strength.
We show how to address this challenge using numerically exact simulation methods by considering two model systems, namely the water-soluble chlorophyll-binding protein of cauliflower and the special pair of bacterial reaction centers.
- Score: 0.0
- License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
- Abstract: The primary steps of photosynthesis rely on the generation, transport, and
trapping of excitons in pigment-protein complexes (PPCs). Generically, PPCs
possess highly structured vibrational spectra, combining many discrete
intra-pigment modes and a quasi-continuous of protein modes, with vibrational
and electronic couplings of comparable strength. The intricacy of the resulting
vibronic dynamics poses significant challenges in establishing a quantitative
connection between spectroscopic data and underlying microscopic models. Here
we show how to address this challenge using numerically exact simulation
methods by considering two model systems, namely the water-soluble
chlorophyll-binding protein of cauliflower and the special pair of bacterial
reaction centers. We demonstrate that the inclusion of the full multi-mode
vibronic dynamics in numerical calculations of linear spectra leads to
systematic and quantitatively significant corrections to electronic parameter
estimation. These multi-mode vibronic effects are shown to be relevant in the
longstanding discussion regarding the origin of long-lived oscillations in
multidimensional nonlinear spectra.
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